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arXiv:1203.2397

Disentangling a quantum antiferromagnet with resonant inelastic X-ray scattering

L. Andrew Wray, Ignace Jarrige, Kazuhiko Ikeuchi, Kenji Ishii, Yuri V. Shvyd'ko, Yuqi Xia, M. Zahid Hasan, Charles Mathy, Hiroshi Eisaki, Jinsheng Wen, Zhijun Xu, Genda D. Gu, Z. Hussain, Yi‐De Chuang

Published Mar 12, 2012• 2 citations
arXivHTMLPDF

Abstract

Low-dimensional copper oxide lattices naturally manifest electronic states with strong short range quantum entanglement, which are known to lead to remarkable emergent material properties. However the nanometer scale many-body wavefunction is challenging to measure or manipulate in a simple way. In this study, X-ray induced $dd$ electronic transitions are used to suppress spin entanglement across a single lattice site in the spin-1/2 antiferromagnetic chain compound SrCuO$_2$, revealing a class of cuprate magnetic excitations that result from breaking the spin chain. These measurements are the first to employ two closely spaced X-ray resonances of copper (M$_2$ and M$_3$) as a form of natural 2-slit interferometer to distinguish between different types of electronic transition and resolve how they influence the dynamics of nearby spin-entangled electrons.

DOI
10.48550/arxiv.1203.2397

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Low-dimensional copper oxide lattices naturally manifest electronic states with strong short range quantum entanglement, which are known to lead to remarkable emergent material properties. However the nanometer scale many-body wavefunction is challenging to measure or manipulate in a simple way. In this study, X-ray induced dddddd electronic transitions are used to suppress spin entanglement across a single lattice site in the spin-1/2 antiferromagnetic chain compound SrCuO2_22​, revealing a class of cuprate magnetic excitations that result from breaking the spin chain. These measurements are the first to employ two closely spaced X-ray resonances of copper (M2_22​ and M3_33​) as a form of natural 2-slit interferometer to distinguish between different types of electronic transition and resolve how they influence the dynamics of nearby spin-entangled electrons.
We report a high-resolution resonant inelastic soft x-ray scattering study of the quantum magnetic spin-chain materials Li(2)CuO(2) and CuGeO(3). By tuning the incoming photon energy to the oxygen K edge, a strong excitation around 3.5 eV energy loss is clearly resolved for both materials. Comparing the experimental data to many-body calculations, we identify this excitation as a Zhang-Rice singlet exciton on neighboring CuO(4) plaquettes. We demonstrate that the strong temperature dependence of the inelastic scattering related to this high-energy exciton enables us to probe short-range spin correlations on the 1 meV scale with outstanding sensitivity.
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Entanglement underpins quantum information processing and computing, yet its experimental quantification in complex, many-body condensed matter systems remains a considerable challenge. Here, we reveal a highly entangled electronic phase proximate to a quantum metal-insulator transition, identified by resonant inelastic x-ray scattering interferometry. This approach reveals that entanglement across atomic sites generates characteristic interference patterns, which our model accurately reproduces, enabling extraction of a full entanglement spectrum and resolution of the underlying quantum states. Our analysis of the pyrochlore iridate Nd2Ir2O7 demonstrates that the system undergoes pronounced quantum fluctuations in its spin, orbital and charge degrees of freedom, even in the presence of a long-range 'all-in-all-out' antiferromagnetic order. Importantly, the observed entanglement signatures facilitate the coexistence of multiple exotic symmetry-breaking orders. Complementary investigations using Raman spectroscopy corroborate the presence of these hidden orders and their emergent excitations. In particular, we observe a two-magnon-bound state below the lowest single-magnon excitation energy, which, together with split phonon modes, provides strong evidence for cubic symmetry-breaking orders of magnetic origin juxtaposed with the all-in-all-out order. Our work thus establishes a direct link between quantum entanglement and emergent unconventional orders, opening new avenues for investigating quantum materials.
Abstract One-dimensional (1D) magnetic insulators have attracted significant interest as a platform for studying quasiparticle fractionalization, quantum criticality, and emergent phenomena. The spin-1/2 Heisenberg chain with antiferromagnetic nearest neighbour interactions is an important reference system; its elementary magnetic excitations are spin-1/2 quasiparticles called spinons that are created in even numbers. However, while the excitation continuum associated with two-spinon states is routinely observed, the study of four-spinon and higher multi-spinon states is an open area of research. Here we show that four-spinon excitations can be accessed directly in Sr2CuO3 using resonant inelastic x-ray scattering (RIXS) in a region of phase space clearly separated from the two-spinon continuum. Our finding is made possible by the fundamental differences in the correlation function probed by RIXS in comparison to other probes. This advance holds promise as a tool in the search for novel quantum states and quantum spin liquids.
Abstract Studying multi-particle elementary excitations has provided unique access to understand collective many-body phenomena in correlated electronic materials, paving the way towards constructing microscopic models. In this work, we perform O K-edge resonant inelastic X-ray scattering (RIXS) on the quasi-one-dimensional cuprate Sr14Cu24O41{{{{{{\rm{Sr}}}}}}}_{14}{{{{{{\rm{Cu}}}}}}}_{24}{{{{{{\rm{O}}}}}}}_{41}Sr14​Cu24​O41​ Sr 14 Cu 24 O 41 with weakly-doped spin ladders. The RIXS signal is dominated by a dispersing sharp mode ~ 270 meV on top of a damped incoherent component ~ 400-500 meV. Comparing with model calculations using the perturbative continuous unitary transformations method, the two components resemble the spin-conserving ΔS = 0 two-triplon bound state and continuum excitations in the spin ladders. Such multi-spin response with long-lived ΔS = 0 excitons is central to several exotic magnetic properties featuring Majorana fermions, yet remains unexplored given the generally weak cross-section with other experimental techniques. By investigating a simple spin-ladder model system, our study provides valuable insight into low-dimensional quantum magnetism.
A recently performed resonant inelastic x-ray scattering experiment (RIXS) at the copper L3{L}_{3}L3​ edge in the quasi-one-dimensional Mott insulator Sr2{}_{2}2​CuO3{}_{3}3​ has revealed a significant dispersion of a single-orbital excitation (orbiton). This large and unexpected orbiton dispersion has been explained using the concept of spin-orbital fractionalization in which the orbiton, which is intrinsically coupled to the spinon in this material, liberates itself from the spinon due to the strictly one-dimensional nature of its motion. Here, we investigate this mechanism in detail by (i) deriving the microscopic spin-orbital superexchange model from the charge-transfer model for the CuO3{}_{3}3​ chains in Sr2{}_{2}2​CuO3{}_{3}3​, (ii) mapping the orbiton motion in the obtained spin-orbital model into a problem of a single hole moving in an effective half-filled antiferromagnetic chain ttt-JJJ model, and (iii) solving the latter model using the exact diagonalization and obtaining the orbiton spectral function. Finally, the RIXS cross section is calculated based on the obtained orbiton spectral function and compared with the RIXS experiment.